EP0170795B1 - Procédé pour récupérer des valeurs d'uranium dans un procédé extractif de retraitement pour matières combustibles nucléaires irradiées - Google Patents

Procédé pour récupérer des valeurs d'uranium dans un procédé extractif de retraitement pour matières combustibles nucléaires irradiées Download PDF

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Publication number
EP0170795B1
EP0170795B1 EP19850105862 EP85105862A EP0170795B1 EP 0170795 B1 EP0170795 B1 EP 0170795B1 EP 19850105862 EP19850105862 EP 19850105862 EP 85105862 A EP85105862 A EP 85105862A EP 0170795 B1 EP0170795 B1 EP 0170795B1
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EP
European Patent Office
Prior art keywords
concentration
fission
uranium
solution
aqueous solution
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Expired - Lifetime
Application number
EP19850105862
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German (de)
English (en)
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EP0170795A2 (fr
EP0170795A3 (en
Inventor
Sameh Abdel Hadi Dr. Ali
Jürgen Dr. Haag
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Forschungszentrum Karlsruhe GmbH
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Kernforschungszentrum Karlsruhe GmbH
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Classifications

    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21C—NUCLEAR REACTORS
    • G21C19/00—Arrangements for treating, for handling, or for facilitating the handling of, fuel or other materials which are used within the reactor, e.g. within its pressure vessel
    • G21C19/42—Reprocessing of irradiated fuel
    • G21C19/44—Reprocessing of irradiated fuel of irradiated solid fuel
    • G21C19/46—Aqueous processes, e.g. by using organic extraction means, including the regeneration of these means
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E30/00—Energy generation of nuclear origin
    • Y02E30/30—Nuclear fission reactors
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
    • Y02W30/00—Technologies for solid waste management
    • Y02W30/50—Reuse, recycling or recovery technologies

Definitions

  • the invention relates to a method for recovering uranium values in an extractive reprocessing process for irradiated nuclear fuels.
  • nuclear reactor fuel elements for recycling irradiated nuclear fuels have been dissolved, for example, in nitric acid and the uranium by liquid / liquid extraction, e.g. in the Purex process or in the amine extraction or in column-chromatographic separation operations, separated and worked up in nitric acid medium.
  • the nitric acid recycling of nuclear fuels is a well-known and proven procedure.
  • the fuel elements to be replaced are removed from the nuclear reactor and, for example, subjected to storage for one to three years to decay the shorter-lived fission products. Only after this period of storage are the fuel elements transported to the reprocessing plant, where they are broken up into relatively small pieces, from which the remaining fission material and the fission products formed, etc. are released with strong nitric acid.
  • the resulting solution is then diluted and passed into a first column in the first extraction cycle of the process, in which an organic extractant solution for taking over the fissile materials uranium and plutonium and smaller amounts of other actinides and small amounts of fission products is passed in countercurrent to the aqueous dissolver solution.
  • the aqueous, nitric acid effluent from the extraction column containing only very small amounts of uranium and plutonium contains the majority of fission products, corrosion products etc. and is a highly radioactive waste solution.
  • the plutonium After washing the organic phase with dilute nitric acid, the plutonium is washed with an aqueous Bring back extraction solution while reducing the oxidation state of the plutonium selectively from the organic phase into the aqueous phase. Thereafter, the uranium still remaining in the organic phase (the majority of the fission materials) is also transferred to an aqueous back-extraction solution.
  • the aqueous solutions of uranium and plutonium are then processed separately, for example with the help of two further cleaning cycles in order to be largely decontaminated from the fission products.
  • the invention has for its object to provide a method with which in an extractive reprocessing process for irradiated nuclear fuel in a process step after the dissolution of the nuclear fuel, no matter at which suitable point in the process, uranium values from one of them, plutonium and fission and Organic extractant solution containing corrosion products can be transferred into an aqueous phase and at the same time separated from plutonium and from the cracking and corrosion products in a simple manner with a relatively high degree of decontamination.
  • the method according to the invention should be applicable in the Purex process and there both in the first extraction cycle and in the uranium cleaning cycles. However, it should also be able to be used in other extraction processes in which uranium values are to be recovered.
  • the aqueous, basic solution containing carbonate ions, with which the organic extractant solution is treated in process step a), can be a maximum of 2.5 molar CO3 ⁇ ions. However, in addition to CO3 ⁇ ions, it can also contain HCO3 ⁇ ions, a maximum of about 1 mol / l.
  • Useful back-extraction solutions of this type have a pH from pH 5 to pH 11.
  • the plutonium can be separated off, for example, by allowing the solution to stand or heating it, with the plutonium oxide hydrate and a subset B (B ⁇ A) of the cleavage products, etc., and then filtering or centrifuging.
  • Any neptunium formed during the irradiation of the uranium in the nuclear reactor follows the path of the uranium in the process according to the invention.
  • the aqueous solution from step c) is adjusted to a ratio of the uranyl ion concentration to carbonate ions / hydrogen carbonate ion concentration of 1: 5 to 1: 8.
  • the aqueous solution from step c) is adjusted at a uranium concentration of 60 g / l to a ratio of UO3++ concentration to CO3 ⁇ / HCO3 ⁇ concentration of 1: 5.
  • a basic anion exchanger such a polyalkene-epoxypolyamine with tertiary amino groups and quaternary ammonium groups of chemical structure RN (CH3) 2 ⁇ HCl and RN+ (CH3) 2 (C2H4OH) Cl ⁇ , where R is the molecule without amino groups, is used.
  • the aqueous solution (step e) advantageously has a hydrogen carbonate ion concentration between 0 and 1 mol / l.
  • the CO3 ⁇ concentration in the aqueous solution (Step e) is at most 2.5 M / l and the pH of the aqueous solution (step e) is in the range from pH 7 to pH 11.
  • the process according to the invention can also be carried out in the absence of HCO3 ⁇ ions, but the process conditions can be set more easily if HCO3 ⁇ ions are present in the aqueous solution.
  • the application of the method spans a large concentration fluctuation range of the uranium stream to be decontaminated. If the uranium concentration in the solution is very small compared to the carbonate concentration, so that, for example, a free CO3 ⁇ / HCO3 ⁇ concentration is higher than 0.6 mol / l, the excess carbonate excess can be optimized either by adding a mineral acid to optimize the fission product retention , preferably HNO3, destroyed or by adding eg Ca (OH) 2 a certain amount of carbonate ions can be trapped.
  • the uranium distribution coefficient must be minimized by adding sufficient amounts of CO3 ⁇ / HCO3 ⁇ ions so that the fission product species are not displaced by the uranium from the ion exchanger.
  • the desired separations can still be carried out at uranium concentrations of approx. 60 g U / l.
  • the limitation of the process to higher U concentrations is due to the uranium solubility in carbonate-hydrogen carbonate solutions.
  • a method for the separation of actinide ions from aqueous, basic, carbonate-containing solutions from German Offenlegungsschrift 31 44 974 was known, in which the actinide ions as carbonate complexes are adsorbed on basic ion exchangers and after separation of the charged ion exchanger from the starting solution with the aid of an aqueous solution are desorbed again by the ion exchanger and processed further, and in which a basic anion exchanger composed of a polyalkene matrix provided with predominantly tertiary amino groups and to a small extent quaternary ammonium groups is also used for the adsorption of the actinide ions, but this method is only meaningfully applicable to aqueous, carbonate-containing waste solutions or washing solutions etc.
  • the main advantages of the method according to the invention are that the decontamination of the uranium from the fission products still present with a relatively small amount of the anion exchanger, e.g. in a relatively small ion exchange column, the ion exchanger loaded with the fission products (with or without a column) can be passed directly to waste treatment and disposal without intermediate treatment.
  • the process according to the invention one or more times on further small anion exchange batches, a high degree of purity of the uranium to be recovered is obtained.
  • the reprocessing and recycling of uranium in the nuclear fuel cycle eliminates the disadvantageous formation of degradation products of the extractant or the diluent in the extraction process.
  • the method according to the invention is characterized by very reliable process control.
  • the organic anion exchanger does not have to be brought into contact with corrosive or strongly oxidizing media in any phase of the process.
  • the method according to the invention works with basic media which offer the highest possible security against the release of volatile iodine components.
  • the solution used in the process according to the invention which can contain up to a maximum of 2.5 mol / l Na2CO3 and at a lower CO3 ⁇ concentration up to approx. 1 mol / l NaHCO3, is chemically very easy to control and radiation-chemical resistant. There are no corrosion problems.
  • the outlay in chemicals, apparatus and working time is very low in the process according to the invention.
  • the average fission product retention during a column run under the specified loading conditions was> 97% for cerium, zirconium and niobium; With ruthenium the retention was about 80%.
  • moderately basic anion exchanger made of polyalkene-epoxypolyamine with tertiary amino and quaternary ammonium groups with the trade name Bio-Rex 5 (from Bio-Rad Laboratories, USA).

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  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • Plasma & Fusion (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Inorganic Compounds Of Heavy Metals (AREA)
  • Extraction Or Liquid Replacement (AREA)

Claims (7)

  1. Procédé de récupération de valeurs d'uranium dans un procédé extractif de retraitement pour matières combustibles nucléaires irradiées, caractérisé en ce que :
    a) la solution d'agent d'extraction organique contenant les substances de fission uranium et plutonium ainsi qu'une quantité partielle (A) des produits de fission et de corrosion provenant de la première étape d'extraction du procédé, est traitée par une solution aqueuse, basique contenant des ions carbonate, dans laquelle les substances de fission et au moins une partie de A sont reextraites dans la phase aqueuse,
    b) les deux phases sont séparés l'une de l'autre,
    c) on élimine de la phase aqueuse d'une manière connue, le plutonium ensemble avec une quantité partielle B des produits de fission d'une manière connue,
    d) la solution aqueuse restante qui contient le complexe carbonate-uranium et une faible quantité résiduelle C de produits de fission est ajustée à un rapport de la concentration en ions uranyl à la concentration en ions carbonate ou à la concentration en CO₃⁻⁻/ HCO₃⁻ de 1(UO₂⁺⁺) à 4,5 (CO₃⁻⁻ ou CO₃⁻⁻/HCO₃) ou en-dessous pour une concentration en U maximale non supérieue à 60 g/litre,
    e) la solution ajustée pour l'adsorption des productions de fission ou des ions renfermant les produits de fission est amenée sur un échangeur d'anions basique à base d'une matrice en polyalcoylène pourvue pour une part prédominante de groupes aminés tertiaires et pour une faible partie de groupes d'ammonium quaternaires et le complexe carbonato-uranyl non adsorbé est récupéré ou décontaminé largement débarrassé de produit de fission.par séparation de la solution uranifère restante de l'échangeur d'ions.
  2. Procédé selon la revendication 1, caractérisé en ce que la solution aqueuse provenant de l'étape c) est ajustée à un rapport de la concentration des ions uranyl à la concentration des ions carbonate/ions hydrogéno-carbonate, de 1:5 à 1:8.
  3. Procédé selon la revendication 1, caractérisé en ce que l'on ajuste la solution aqueuse provenant de l'étape c) pour une concentration en U de 60 g/l, à un rapport de la concentration en UO₂⁺⁺/à la concentration en CO₃⁻⁻/HCO₃⁻ de 1:5.
  4. Procédé selon la revendication 1, caractérisé en ce que comme échangeur d'anions basique, on utilise celui à base de polyalcoylène-époxypolyamine avec des groupes aminés tertiaires et des groupes d'ammonium quaternaires de structure chimique R-N(+)(CH₃)₂ (C₂H₄OH) Cl(-) dans lesquelles R représente la molécule sans groupe aminé.
  5. Procédé selon la revendication 1, caractérisé en ce que la solution aqueuse (étape e) a une concentration des ions hydrogénocarbonates comprise entre 0 et 1 mole/l.
  6. Procédé selon la revendication 1, caractérisé en ce que la concentration en CO₃⁻⁻ dans la solution aqueuse (étape e) se monte au maximum à 2,5 mole/l.
  7. Procédé selon la revendication 1, caractérisé en ce que la valeur de pH de la solution aqueuse ajustée (étape e) se situe dans la gamme de pH 7 à pH 11.
EP19850105862 1984-08-04 1985-05-13 Procédé pour récupérer des valeurs d'uranium dans un procédé extractif de retraitement pour matières combustibles nucléaires irradiées Expired - Lifetime EP0170795B1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE3428878 1984-08-04
DE19843428878 DE3428878A1 (de) 1984-08-04 1984-08-04 Verfahren zur rueckgewinnung von uran-werten in einem extraktiven wiederaufarbeitungsprozess fuer bestrahlte kernbrennstoffe

Publications (3)

Publication Number Publication Date
EP0170795A2 EP0170795A2 (fr) 1986-02-12
EP0170795A3 EP0170795A3 (en) 1989-01-04
EP0170795B1 true EP0170795B1 (fr) 1992-09-09

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EP19850105862 Expired - Lifetime EP0170795B1 (fr) 1984-08-04 1985-05-13 Procédé pour récupérer des valeurs d'uranium dans un procédé extractif de retraitement pour matières combustibles nucléaires irradiées

Country Status (4)

Country Link
US (1) US4740359A (fr)
EP (1) EP0170795B1 (fr)
JP (1) JPH0631803B2 (fr)
DE (1) DE3428878A1 (fr)

Families Citing this family (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE3708751C2 (de) * 1987-03-18 1994-12-15 Kernforschungsz Karlsruhe Verfahren zur nassen Auflösung von Uran-Plutonium-Mischoxid-Kernbrennstoffen
US7097747B1 (en) 2003-08-05 2006-08-29 Herceg Joseph E Continuous process electrorefiner
DE102004050308A1 (de) 2004-10-14 2006-06-14 Framatome Anp Gmbh Verfahren und Probenahmesystem zur Gewinnung einer Probe aus der Atmosphäre in einem Reaktorsicherheitsbehälter einer kerntechnischen Anlage
US20090022638A1 (en) * 2007-07-19 2009-01-22 Duilio Rossoni Ion exchanger for winning metals of value
CA2684774A1 (fr) 2007-12-05 2009-06-18 Alltech Associates, Inc. Procedes et appareils d'analyse d'echantillons et de prelevement de fractions d'echantillons
US8066861B1 (en) 2008-02-14 2011-11-29 The United States Of America As Represented By The Department Of Energy Method for preparing metal powder, device for preparing metal powder, method for processing spent nuclear fuel
US8314934B2 (en) 2009-09-01 2012-11-20 Alltech Associates, Inc. Methods and apparatus for analyzing samples and collecting sample fractions
CN112403032A (zh) * 2020-11-18 2021-02-26 中国核动力研究设计院 一种均匀性水溶液核反应堆燃料溶液中99Mo、131I共提取的方法

Family Cites Families (11)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2768871A (en) * 1945-07-30 1956-10-30 Harrison S Brown Process using carbonate precipitation
US2767044A (en) * 1947-12-02 1956-10-16 Orville F Hill Plutonium recovery process
US2811412A (en) * 1952-03-31 1957-10-29 Robert H Poirier Method of recovering uranium compounds
US3155455A (en) * 1960-12-12 1964-11-03 Phillips Petroleum Co Removal of vanadium from aqueous solutions
US3864667A (en) * 1970-09-11 1975-02-04 Continental Oil Co Apparatus for surface wave parameter determination
US3835044A (en) * 1972-10-16 1974-09-10 Atomic Energy Commission Process for separating neptunium from thorium
US3922231A (en) * 1972-11-24 1975-11-25 Ppg Industries Inc Process for the recovery of fission products from waste solutions utilizing controlled cathodic potential electrolysis
US4280985A (en) * 1979-03-16 1981-07-28 Mobil Oil Corporation Process for the elution of ion exchange resins in uranium recovery
US4423008A (en) * 1979-10-01 1983-12-27 Mobil Oil Corporation Direct acid elution of anionic exchange resins for recovery of uranium
DE3144974C2 (de) * 1981-11-12 1986-01-09 Kernforschungszentrum Karlsruhe Gmbh, 7500 Karlsruhe Verfahren zur Abtrennung von Aktinoidenionen aus wäßrigen, basischen, carbonathaltigen Lösungen
DE3428877A1 (de) * 1984-08-04 1986-02-13 Kernforschungszentrum Karlsruhe Gmbh, 7500 Karlsruhe Verfahren zur trennung von grossen mengen uran von geringen mengen von radioaktiven spaltprodukten, die in waessrigen basischen, karbonathaltigen loesungen vorliegen

Also Published As

Publication number Publication date
EP0170795A2 (fr) 1986-02-12
JPH0631803B2 (ja) 1994-04-27
US4740359A (en) 1988-04-26
DE3428878C2 (fr) 1993-01-21
EP0170795A3 (en) 1989-01-04
JPS6141994A (ja) 1986-02-28
DE3428878A1 (de) 1986-02-13

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